Design of stable mixed-metal MIL-101(Cr/Fe) materials with enhanced catalytic activity for the Prins reaction

Cristina Vallés-García; Effrosyni Gkaniatsou; Andrea Santiago-Portillo; Mónica Giménez-Marqués; Mercedes Álvaro; Jean Marc Greneche; Nathalie Steunou; Clémence Sicard; Sergio Navalón; Christian Serre; Hermenegildo García

doi:10.1039/d0ta02991b

Design of stable mixed-metal MIL-101(Cr/Fe) materials with enhanced catalytic activity for the Prins reaction

Cristina Vallés-García, Effrosyni Gkaniatsou, Andrea Santiago-Portillo, Mónica Giménez-Marqués, Mercedes Álvaro, Jean Marc Greneche, Nathalie Steunou, Clémence Sicard, Sergio Navalón, Christian Serre, Hermenegildo García

Résultats de recherche: Contribution à un journal/une revue › Article › Revue par des pairs

Résumé

This work highlights the benefit of designing mixed-metal (Cr/Fe) MOFs for enhanced chemical stability and catalytic activity. A robust and stable mixed-metal MIL-101(Cr/Fe) was prepared through a HF-free direct hydrothermal route with Fe3+ content up to 21 wt%. The incorporation of Fe3+ cations in the crystal structure was confirmed by 57Fe Mössbauer spectrometry. The catalytic performance of the mixed metal MIL-101(Cr/Fe) was evaluated in the Prins reaction. MIL-101(Cr/Fe) exhibited a higher catalytic activity compared to MIL-101(Cr), improved chemical stability compared to MIL-101(Fe) and a higher catalytic activity for bulky substrates compared to MIL-100(Fe). In situ infra-red spectroscopy study suggests that the incorporation of Fe3+ ions in MIL-101 structure leads to an increase in Lewis acid sites. It was thus concluded that the predominant role of Cr3+ ions was to maintain the crystal structure, while Fe3+ ions enhanced the catalytic activity.

langue originale	Anglais
Pages (de - à)	17002-17011
Nombre de pages	10
journal	Journal of Materials Chemistry A
Volume	8
Numéro de publication	33
Les DOIs	https://doi.org/10.1039/d0ta02991b
Etat de la publication	Publié - 7 sept. 2020
Modification externe	Oui

Financement

Financial support by the Spanish Ministry of Economy and Competitiveness (Severo Ochoa, CTQ2018-890237-CO2-R1 and Maria de Maeztu, CEX2019-000919-M), is gratefully acknowledged. Generalidad Valenciana is also thanked for funding (Prometeo 2017/083). S. N. thanks nancial support by the Min-isterio de Ciencia, Innovación y Universidades (RTI 2018-099482-A-I00 project), Fundación Ramón Areces (XVIII Concurso Nacio-nal para la Adjudicación de Ayudas a la Investigación en Ciencias de la Vida y de la Materia, 2016), and Generalitat Valenciana grupos de investigación consolidables 2019 (ref: AICO/2019/214) project. E. G. thanks the ANR-11-LABEX-0039 (LabEx CHARM3AT) for nancial support. M. G.-M thanks support from “la Caixa” Foundation (LCF/BQ/PI19/11690022) and Generalitat Valenciana (SEJI/2020/036).

Bailleurs de fonds	Numéro du bailleur de fonds
Fundación Ramón Areces
Generalitat Valenciana	AICO/2019/214
Generalitat Valenciana
Investigación en Ciencias de la Vida y de la Materia
“la Caixa” Foundation	SEJI/2020/036, LCF/BQ/PI19/11690022
“la Caixa” Foundation
Ministerio de Economía y Competitividad	2017/083, CEX2019-000919-M, CTQ2018-890237-CO2-R1
Ministerio de Economía y Competitividad
Ministerio de Ciencia, Innovación y Universidades	RTI 2018-099482-A-I00
Ministerio de Ciencia, Innovación y Universidades

SDG des Nations Unies

Ce résultat contribue à ou aux Objectifs de développement durable suivants

Accès au document

10.1039/d0ta02991b

Autres fichiers et liens

Link to publication in Scopus

Contient cette citation

Vallés-García, C., Gkaniatsou, E., Santiago-Portillo, A., Giménez-Marqués, M., Álvaro, M., Greneche, J. M., Steunou, N., Sicard, C., Navalón, S., Serre, C., & García, H. (2020). Design of stable mixed-metal MIL-101(Cr/Fe) materials with enhanced catalytic activity for the Prins reaction. Journal of Materials Chemistry A, 8(33), 17002-17011. https://doi.org/10.1039/d0ta02991b

@article{634ba610522041aaa850345abe710018,

title = "Design of stable mixed-metal MIL-101(Cr/Fe) materials with enhanced catalytic activity for the Prins reaction",

abstract = "This work highlights the benefit of designing mixed-metal (Cr/Fe) MOFs for enhanced chemical stability and catalytic activity. A robust and stable mixed-metal MIL-101(Cr/Fe) was prepared through a HF-free direct hydrothermal route with Fe3+ content up to 21 wt%. The incorporation of Fe3+ cations in the crystal structure was confirmed by 57Fe M{\"o}ssbauer spectrometry. The catalytic performance of the mixed metal MIL-101(Cr/Fe) was evaluated in the Prins reaction. MIL-101(Cr/Fe) exhibited a higher catalytic activity compared to MIL-101(Cr), improved chemical stability compared to MIL-101(Fe) and a higher catalytic activity for bulky substrates compared to MIL-100(Fe). In situ infra-red spectroscopy study suggests that the incorporation of Fe3+ ions in MIL-101 structure leads to an increase in Lewis acid sites. It was thus concluded that the predominant role of Cr3+ ions was to maintain the crystal structure, while Fe3+ ions enhanced the catalytic activity. ",

author = "Cristina Vall{\'e}s-Garc{\'i}a and Effrosyni Gkaniatsou and Andrea Santiago-Portillo and M{\'o}nica Gim{\'e}nez-Marqu{\'e}s and Mercedes {\'A}lvaro and Greneche, {Jean Marc} and Nathalie Steunou and Cl{\'e}mence Sicard and Sergio Naval{\'o}n and Christian Serre and Hermenegildo Garc{\'i}a",

note = "Funding Information: Financial support by the Spanish Ministry of Economy and Competitiveness (Severo Ochoa, CTQ2018-890237-CO2-R1 and Maria de Maeztu, CEX2019-000919-M), is gratefully acknowledged. Generalidad Valenciana is also thanked for funding (Prometeo 2017/083). S. N. thanks nancial support by the Min-isterio de Ciencia, Innovaci{\'o}n y Universidades (RTI 2018-099482-A-I00 project), Fundaci{\'o}n Ram{\'o}n Areces (XVIII Concurso Nacio-nal para la Adjudicaci{\'o}n de Ayudas a la Investigaci{\'o}n en Ciencias de la Vida y de la Materia, 2016), and Generalitat Valenciana grupos de investigaci{\'o}n consolidables 2019 (ref: AICO/2019/214) project. E. G. thanks the ANR-11-LABEX-0039 (LabEx CHARM3AT) for nancial support. M. G.-M thanks support from “la Caixa” Foundation (LCF/BQ/PI19/11690022) and Generalitat Valenciana (SEJI/2020/036). Publisher Copyright: {\textcopyright} 2020 The Royal Society of Chemistry. Copyright: Copyright 2020 Elsevier B.V., All rights reserved.",

year = "2020",

month = sep,

day = "7",

doi = "10.1039/d0ta02991b",

language = "English",

volume = "8",

pages = "17002--17011",

journal = "Journal of Materials Chemistry A",

issn = "2050-7488",

publisher = "Royal Society of Chemistry",

number = "33",

}

Vallés-García, C, Gkaniatsou, E, Santiago-Portillo, A, Giménez-Marqués, M, Álvaro, M, Greneche, JM, Steunou, N, Sicard, C, Navalón, S, Serre, C & García, H 2020, 'Design of stable mixed-metal MIL-101(Cr/Fe) materials with enhanced catalytic activity for the Prins reaction', Journal of Materials Chemistry A, VOL. 8, Numéro 33, p. 17002-17011. https://doi.org/10.1039/d0ta02991b

Design of stable mixed-metal MIL-101(Cr/Fe) materials with enhanced catalytic activity for the Prins reaction. / Vallés-García, Cristina; Gkaniatsou, Effrosyni; Santiago-Portillo, Andrea et al.
Dans: Journal of Materials Chemistry A, Vol 8, Numéro 33, 07.09.2020, p. 17002-17011.

Résultats de recherche: Contribution à un journal/une revue › Article › Revue par des pairs

TY - JOUR

T1 - Design of stable mixed-metal MIL-101(Cr/Fe) materials with enhanced catalytic activity for the Prins reaction

AU - Vallés-García, Cristina

AU - Gkaniatsou, Effrosyni

AU - Santiago-Portillo, Andrea

AU - Giménez-Marqués, Mónica

AU - Álvaro, Mercedes

AU - Greneche, Jean Marc

AU - Steunou, Nathalie

AU - Sicard, Clémence

AU - Navalón, Sergio

AU - Serre, Christian

AU - García, Hermenegildo

N1 - Funding Information: Financial support by the Spanish Ministry of Economy and Competitiveness (Severo Ochoa, CTQ2018-890237-CO2-R1 and Maria de Maeztu, CEX2019-000919-M), is gratefully acknowledged. Generalidad Valenciana is also thanked for funding (Prometeo 2017/083). S. N. thanks nancial support by the Min-isterio de Ciencia, Innovación y Universidades (RTI 2018-099482-A-I00 project), Fundación Ramón Areces (XVIII Concurso Nacio-nal para la Adjudicación de Ayudas a la Investigación en Ciencias de la Vida y de la Materia, 2016), and Generalitat Valenciana grupos de investigación consolidables 2019 (ref: AICO/2019/214) project. E. G. thanks the ANR-11-LABEX-0039 (LabEx CHARM3AT) for nancial support. M. G.-M thanks support from “la Caixa” Foundation (LCF/BQ/PI19/11690022) and Generalitat Valenciana (SEJI/2020/036). Publisher Copyright: © 2020 The Royal Society of Chemistry. Copyright: Copyright 2020 Elsevier B.V., All rights reserved.

PY - 2020/9/7

Y1 - 2020/9/7

N2 - This work highlights the benefit of designing mixed-metal (Cr/Fe) MOFs for enhanced chemical stability and catalytic activity. A robust and stable mixed-metal MIL-101(Cr/Fe) was prepared through a HF-free direct hydrothermal route with Fe3+ content up to 21 wt%. The incorporation of Fe3+ cations in the crystal structure was confirmed by 57Fe Mössbauer spectrometry. The catalytic performance of the mixed metal MIL-101(Cr/Fe) was evaluated in the Prins reaction. MIL-101(Cr/Fe) exhibited a higher catalytic activity compared to MIL-101(Cr), improved chemical stability compared to MIL-101(Fe) and a higher catalytic activity for bulky substrates compared to MIL-100(Fe). In situ infra-red spectroscopy study suggests that the incorporation of Fe3+ ions in MIL-101 structure leads to an increase in Lewis acid sites. It was thus concluded that the predominant role of Cr3+ ions was to maintain the crystal structure, while Fe3+ ions enhanced the catalytic activity.

AB - This work highlights the benefit of designing mixed-metal (Cr/Fe) MOFs for enhanced chemical stability and catalytic activity. A robust and stable mixed-metal MIL-101(Cr/Fe) was prepared through a HF-free direct hydrothermal route with Fe3+ content up to 21 wt%. The incorporation of Fe3+ cations in the crystal structure was confirmed by 57Fe Mössbauer spectrometry. The catalytic performance of the mixed metal MIL-101(Cr/Fe) was evaluated in the Prins reaction. MIL-101(Cr/Fe) exhibited a higher catalytic activity compared to MIL-101(Cr), improved chemical stability compared to MIL-101(Fe) and a higher catalytic activity for bulky substrates compared to MIL-100(Fe). In situ infra-red spectroscopy study suggests that the incorporation of Fe3+ ions in MIL-101 structure leads to an increase in Lewis acid sites. It was thus concluded that the predominant role of Cr3+ ions was to maintain the crystal structure, while Fe3+ ions enhanced the catalytic activity.

UR - http://www.scopus.com/inward/record.url?scp=85090587338&partnerID=8YFLogxK

U2 - 10.1039/d0ta02991b

DO - 10.1039/d0ta02991b

M3 - Article

AN - SCOPUS:85090587338

SN - 2050-7488

VL - 8

SP - 17002

EP - 17011

JO - Journal of Materials Chemistry A

JF - Journal of Materials Chemistry A

IS - 33

ER -

Design of stable mixed-metal MIL-101(Cr/Fe) materials with enhanced catalytic activity for the Prins reaction

Résumé

Financement

SDG des Nations Unies

Accès au document

Autres fichiers et liens

Empreinte digitale

Contient cette citation